A series of crystalline mesoporous molecular sieves were prepared using alkyl hexadecyl dimethyl ammonium bromide salts (C16H33)(CnH2n + 1)(CH3)2NBr, in which the number of carbon atoms (n) in one alkyl group was varied from 1 to 12. The influence of (n) value on the nature of the final phase obtained and on its pore size was investigated. A hexagonal phase was obtained for n = 1, 3, 5 and 7, while a lamellar phase was obtained for all other templates. Vanadium and titanium modified MCM-41 molecular sieves were also prepared in the presence of C12H25(CH3)3N+ and C16H33(CH3)3N+ ions, respectively. These materials were characterized by XRD, nitrogen physisorption, FTIR, solid state NMR, XPS, UV-Vis and catalytic testing in the oxidation of 1-naphthol, 2,6-di-tert-butylphenol, norbornylene, n-hexane and propylamine. Ti-MCM-41 exhibited considerable catalytic activity only in the oxidation of aromatics, olefins and alcohols. V-MCM-41 was found to be a good catalyst in the oxidation of aromatics and alkanes.